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Cumulative short-lived photofission product yields for nuclear forensic application

Experiments have long been carried out with linear accelerator (linac) produced bremsstrahlung X-rays to study high-energy photon-induced fission, known as “photofission”. One benefit of photofission, when compared with neutron-induced fission, is the ability to investigate fundamental physics of fission at excitation energies lower than what is possible with neutrons [1]. Absorption of an incident neutron results in a compound nucleus with an excitation energy at least equal to the neutron binding energy; thus, the lowest energy region of the fission barrier cannot be studied. Fission product yield distributions are dependent on the incident particle energy and the target nucleus mass. They are generally represented by a double-humped curve, with low and high mass “peaks” and an intermediate mass “valley”. As incident particle energy increases, the excitation energy of the nucleus increases, thereby increasing the overall yield of isotopes in the valley with respect to the two maxima or peaks of the fission product curve [3]. Photofission is most probable for incident photons around 14 MeV due to the giant dipole resonance. Induced photofission around this energy results in a fission product yield distribution that resembles 14 MeV DT neutron fission more than thermal or fast (500 keV) neutron fission. In post-detonation nuclear forensics, the peak-to-valley ratio of the fission product yield curve could be used for characterizing device type by providing an indication of the neutron energy spectrum that had induced fission (e.g., 500 keV vs. 14 MeV). The goal of this work is to improve nuclear data for isotopes of interest in nuclear forensics and special nuclear material (SNM) detection, specifically the fission product yield data via photofission experiments for the isotopes of 238U and 232Th. Photofission has been proposed as a less costly and more flexible production method for the valley isotopes that are representative of DT neutron fission product yield distributions, which would benefit nuclear forensics exercises in testing for analysis techniques. Natural uranium and thorium targets were irradiated with bremsstrahlung photons (nominal endpoint energies of 8, 14, and 20 MeV), generated via impingement of high-energy electrons on a tungsten electron-to-photon radiator. Gamma-ray spectroscopy was used to observe and identify the decay of the resulting fission products. The photofission yields of 102 fission products were measured for the set of the 238U and 232Th targets at the three bremsstrahlung X-ray endpoint energies 8, 14, and 20 MeV. These fragments included masses ranging from A=84 to A=144, with half-lives as short as 1.07 seconds.

07 ISOTOPE AND RADIATION SOURCES↗

Photofission Validation Measurements for Active Interrogation Standards

Executive Summary PNNL has been developing technical standards for the detection of special nuclear material (SNM) in cargo containers using active interrogation approaches. Since the use of kilogram-scale quantities of SNM is impractical for standards testing, the work focused on designing surrogates that provided similar signature as the SNM. There are many active interrogation approaches to detect SNM; the standards development considered photofission, differential die-away and nuclear resonance fluorescence. Of these approaches, photofission currently carries the most interest. However, uncertainties in the photofission cross sections are as large as 50%, so that validation measurements are necessary to provide confidence that the surrogate will perform similarly to the SNM. This document describes approaches for conducting those validation measurements as well as provides a rough order-of-magnitude cost estimate for performing them. Photofission provides many observables for the detection of SNM. The standards development considered prompt neutrons, delayed neutrons and delayed gamma rays as possible detected particles. The surrogates, which consist primarily of depleted uranium (DU), were designed to reproduce the strength of these particles for a targeted quantity of 2 kg of HEU. Different surrogates are required for different measurement approaches because of the difference in cross section between 235 U and 238 U. For the standards validations, the relative strength of the detected particles for HEU and DU must be measured. To avoid measurements with kilogram-sized SNM, the validation approach is focused on two comparisons. In the first comparison, the relative rates for approximately 10 g samples of DU and HEU will be measured. This comparison will provide the basis for validating the relative strength of the detected particles for HEU and DU. In the second comparison, the relative rates for the approximately 10 g and 1 kg sample of DU will be measured. This comparison will enable the validation of secondary processes that occur after photofission that impact the measurement for kilogram-scale samples. For instance, for 2 kg of HEU, as much as 50% of the fission induced in the sample is induced from fission neutrons generated through photofission. There is a limited range of facilities in the U.S. that have both the necessary accelerator capability and the ability and willingness to handle SNM. Two such facilities, the Idaho Accelerator Center at Idaho State University and the Nuclear Engineering Program at the University of Michigan, have both expressed an interest in participating in such measurements. Both would need to amend their licensing to handle the 10 g of HEU proposed for these measurements. The rough order-of-magnitude cost estimate for all three validation measurements is $1.1M, spread over three years. Each of the three measurements could be performed separately, at approximately one-third of that cost. There are a number of critical assumptions in these cost estimate that will need to be confirmed before a more reliable cost estimate can be established. PNNL will manage the effort to ensure that the overall objective of the validation measurements can be achieved and will fabricate the 10 g samples of HEU and DU. Most the labor for the measurements will be provided by two collaborating universities as research opportunities for students. The successful completion of these validation measurements will reduce the uncertainties in the proposed standards from about 50% to 5%. The measurements would also provide some much-needed nuclear data on photofission.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Neutron-Neutron Correlations in the Photofission of 238U

Background: In the fission of actinides, the nearly back-to-back motion of the fission fragments has a strong effect on the kinematics of fission neutrons. This leads to a favoring of opening angles near 0? and 180? in the neutron-neutron (n-n) opening angle distributions of correlated neutron pairs from the same fission event. Purpose: To measure the n-n opening angle and energy correlations in the photofission of 238U. As of this writing, measurements of correlated n-n opening angle distributions have been reported only for the spontaneous and neutron-induced fission of actinides. This work is the first to report such a measurement using photofission and will provide useful experimental input for photofission models used in codes such as MCNP and FREYA. Method: Fission is induced using bremsstrahlung photons produced via a low duty factor, pulsed, linear electron accelerator. The bremsstrahlung photon beam impinges upon a 238U target that is surrounded by a large neutron scintillation detection system capable of measuring particle position and time of flight, from which n-n opening angle and energy are measured. Neutron-neutron angular correlations are determined by taking the ratio between a correlated neutron distribution and an uncorrelated neutron distribution formed by the pairing of neutrons produced during different beam pulses. This analysis technique greatly diminishes effects due to detector efficiencies, acceptance, and experimental drifts. Results: The angular correlation of neutrons from the photofission of 238U shows a high dependence on neutron energy as well as a dependence on the angle of the emitted neutrons with respect to the incoming photon beam. Angular correlations were also measured using neutrons from the spontaneous fission of 252Cf, showing good agreement with past measurements. Conclusions: The measured angular correlations reflect the underlying back-to-back nature of the fission fragments. An anomalous decline in n-n yield was observed for opening angles near 180? for 238U.

Burggraf, Jeff↗

Near-barrier photofission in Th 232 and U 238

Here a study of photofission of $^{232}\mathrm{Th}$ and $^{238}\mathrm{U}$ was performed by using quasimonoenergetic, linearly polarized ${\gamma}$-ray beams from the High Intensity ${\gamma}$-ray Source at Triangle Universities Nuclear Laboratory. The prompt-photofission neutron polarization asymmetries, neutron multiplicities, and the photofission cross sections were measured in the near-barrier energy range of 4.3 to 6.0 MeV. This data set constitutes the lowest energy measurements of those observables to date using quasimonoenergetic photons. Large polarization asymmetries are observed in both nuclei, consistent with the $E1$ excitation as observed by another measurement of this kind made in a higher-energy range. Previous experimental evidence of a deep third minimum in the $^{238}\mathrm{U}$ fission barrier has been identified as an accelerator-induced background.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Delayed Neutrons from Photofission of {sup 238}U at E{sub γ} ≲ 10 MeV

— The technique is described for measuring energy spectra and temporal distributions of delayed neutrons from photofission at the pulsed electron accelerator LUE-8-5 of the Institute for Nuclear Research of the Russian Academy of Sciences (INR RAS). The measurements were performed by the neutron scintillation spectrometer using pulse shape discrimination of background γ-quanta. The results of measurements of {sup 238}U-photofission with the kinetic energy of incident electrons ≈10 MeV are given.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Measurement of the Delayed Photon Yield of the Photofission Reaction as a Method for Identifying Fissile Materials

The results of measuring the photofission reaction yield for actinide nuclei in the near-threshold energy region are presented. At the LUE-8-5 accelerator of the Institute for Nuclear Research of the Russian Academy of Sciences, the energy and time spectra of the delayed gamma quanta were obtained by irradiating fissile isotopes by bremsstrahlung photons. The conclusion is drawn about the possibility of identifying fissile isotopes by the behavior of the photofission cross section in the near-threshold region.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Prompt Photofission Neutron Detection in Depleted Uranium

The detection of prompt photofission neutrons during active interrogation is a strong indication of the presence of special nuclear materials. However, the high-energy photons used for interrogation create a very challenging radiation environment for the detection of prompt fission signatures. These challenges include detector saturation and pulse pile-up. Additionally, there is an elevated neutron background that further challenges the detection of prompt fission neutrons. This background is produced because of (γ, Xn) photonuclear reactions in the surrounding high-Z materials. Here, we demonstrate the detection of prompt photofission neutrons in these challenging environments. Depleted uranium (DU) and lead targets are interrogated with bremsstrahlung photons produced by a 9-MV electron linear accelerator. Fast neutrons are detected with trans-stilbene organic detectors, and scintillation pulses are analyzed using a previously developed and demonstrated artificial neural network system. We observe a 5 times higher photoneutron count rate when the lead target is replaced with the DU target. Additionally, we observe a difference in the photoneutron light-output distributions of lead and DU. Here, this difference in the measured distributions is due to the difference in the photoneutron-energy spectra; DU photoneutrons are emitted with (γ, n) and watt-energy spectra, whereas lead photoneutrons are emitted with only the (γ, n) spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Detection of uranium-photofission neutrons with a 4 He scintillation detector

The use of photon active interrogation to detect special nuclear material has held significant theoretical promise, as the interrogating source particles, photons, are fundamentally different from one of the main signatures of special nuclear material: neutrons produced in nuclear fission. However, neutrons produced by photonuclear reactions in the accelerator target, collimator, and environment can obscure the fission neutron signal. These (γ, n) neutrons could be discriminated from fission neutrons by their energy spectrum, but common detectors sensitive to the neutron spectrum, like organic scintillators, are typically hampered by the intense photon background characteristic of photon-based active interrogation. In contrast, high-pressure 4 ⁢He-based scintillation detectors are well-suited to photon active interrogation, as they are similarly sensitive to fast neutrons and can measure their spectrum, but show little response to gamma rays. Here, in this work, a photon active interrogation system utilizing a 4 ⁢He scintillation detector and a 9 MeV linac-bremsstrahlung x-ray source was experimentally evaluated. The detector was shown to be capable of operating in intense gamma-ray environments and detecting photofission neutrons from 238 ⁢U when interrogated by this x-ray source. The photofission neutrons show clear spectral separation from (γ, n) neutrons produced in lead, a common shielding material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Short-lived photofission product yields from 238 U and 232 Th at Bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV for nuclear forensics isotope production applications

The existing photofission product yield data sets are often based on nuclear models, and limited experimental measurements of these fission product yields have been performed. These experiments resulted in measured cumulative fission product yields (CFPYs) for 238 U and 232 Th for the bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV. The half-lives of the reported fission products range from 1.07–40.8 s. This work is motivated by a demonstrated need for novel isotope production methods for nuclear forensics and improved nuclear data to support the nonproliferation community. A high-purity germanium detector and a pneumatic transfer system were employed for measurements of short-lived fission products, collecting data between cycles of accelerator irradiation and measurement.

07 ISOTOPE AND RADIATION SOURCES↗

Photofission cross-section ratio measurement of 235 U/ 238 U using monoenergetic photons in the energy range of 9.0–16.6 MeV

Photofission cross-section ratios of 235U and 238U have been measured using monoenergetic photon beams from the High Intensity Gamma-ray Source facility at the Triangle Universities Nuclear Laboratory. These measurements have been performed in small energy steps between 9.0 and 16.6 MeV using a dual-fission ionization chamber. The measured cross-section ratios are compared with the previous experimental data as well as with the recent evaluated nuclear data library ENDF.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Exploratory study of fission product yield determination from photofission of Pu 239 at 11 MeV with monoenergetic photons

Here, measurements of fission product yields play an important role for the understanding of fundamental aspects of the fission process. Recently, neutron-induced fission product-yield data of 239 Pu at energies below 4 MeV revealed an unexpected energy dependence of certain fission fragments. In order to investigate whether this observation is prerogative to neutron-induced fission, a program has been initiated to measure fission product yields in photoinduced fission. Here we report on the first ever photofission product yield measurement with monoenergetic photons produced by Compton back-scattering of FEL photons. The experiment was performed at the High-Intensity Gamma-ray Source at Triangle Universities Nuclear Laboratory on 239 Pu at E γ = 11 MeV. In this exploratory study the yield of eight fission products ranging from 91 Sr to 143 Ce has been obtained.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fissile material detection using neutron time-correlations from photofission

The detection of special nuclear materials (SNM) in commercial cargoes is a major objective in the field of nuclear security. In this work we investigate the use of two-neutron time-correlations from photo-fission using the Prompt Neutrons from Photofission (PNPF) detectors in Passport Systems Inc.’s (PSI) Shielded Nuclear Alarm Resolution (SNAR) platform for the purpose of detecting ~5 kg quantities of fissionable materials in seconds. The goal of this effort was to extend the secondary scan mode of this system to differentiate fissile materials, such as highly enriched uranium, from fissionable materials, such as low enriched and depleted uranium (LEU and DU). Experiments were performed using a variety of material samples, and data were analyzed using the variance-over-mean technique referred to as Y 2F or Feynman-α. Results were compared to computational models to improve our ability to predict system performance for distinguishing fissile materials. Simulations were then combined with empirical formulas to generate receiver operating characteristics (ROC) curves for a variety of shielding scenarios. We show that a 10 second screening with a 200 μA 9 MeV X-ray beam is sufficient to differentiate kilogram quantities of HEU from DU in various shielding scenarios in a standard cargo container.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Measurements of Short-Lived Isomers from Photofission as a Method of Active Interrogation for Special Nuclear Materials

Isomeric fission products, such as 134m Te (T 1/2 = 164 ns) and 136m Xe (T 1/2 = 2.95 μs), are proposed as a signature of special nuclear materials in active interrogation applications. To test this conjecture, monoenergetic 9, 11, and 13 MeV photons from the HIγS facility are used to induce fission of 235 U, 238 U, and 239 Pu targets. The de-excitation γ rays of the isomers are measured using time-gated spectroscopy with high-purity germanium detectors. The 134m Te and 136m Xe isomers are detected and identified by the energy and decay half-life of their characteristic γ-ray transitions. The ratio of yields for these two signature γ rays, corresponding to 134m Te/( 136m Xe + 136 I), is found to be strongly correlated with the identity of the fissioning nuclei. These results show that fission-product isomers may be used in active interrogation to detect and identify special nuclear materials, even providing information on the isotopic enrichment. In conclusion, the feasibility of an active interrogation scenario using a bremsstrahlung beam is discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurements of short-lived fission product yields from photofission of 238 U using 13.0 MeV monoenergetic photons

Photon-induced fission product yield (FPY) measurements were conducted on the isotope 238U. Fission was induced using Eγ = 13.0 MeV monoenergetic photons produced by the Triangle Universities Nuclear Laboratory’s (TUNL’s) High Intensity γ-ray Source (HIγS) facility. Short-lived FPYs were measured by performing cyclic activation of the sample using a rapid target transfer system. Following activation, the 238U target was rapidly (0.4 s) transferred to a counting station consisting of two well-shielded high-purity germanium (HPGe) detectors. The irradiation-counting cycle was repeated until the summed data had sufficient statistical accuracy. Twenty-eight unique fission products with half-lives ranging from 1 s to 450 s were identified, and their cumulative FPYs determined. Furthermore, the results are compared with previous independent FPY measurements using inverse kinematics. Good agreement between the data sets is found despite the different excitation energy distributions of the fissioning nucleus in the experiments.

Physics - Nuclear physics and radiation physics↗